2D molecular crystals (2DMCs) are emerging as excellent candidates for the application of organic field‐effect transistors (OFETs), owing to their enhanced charge transport efficiency and long‐range molecular ordering. However, many current methods involve an additional transfer process, which largely hinders the large‐area fabrication of high‐quality, intact 2DMCs for practical applications. Here, an efficient surficial Marangoni flow‐induced self‐assembly (SMFIS) method is developed for the fabrication of 2DMCs directly on target substrates without the need of a transfer process. This method utilizes a solvent/antisolvent system to confine the crystallization field at a liquid/air interface, and then the formed 2DMCs land on the target substrate with the full solvent evaporation. By controlling the vertical convection flow and the spreading coefficient of the solvent/antisolvent system, few‐layer (3–4 layers) 2DMCs are directly produced on the target substrates. The SMFIS method shows no substrate dependency and universal compatibility. With bis(triethylsilylethynyl)anthradithiophene (Dif‐TES‐ADT) as an example, the resulting 2D Dif‐TES‐ADT crystal exhibits an efficient charge transport with high average mobility up to 2.15 cm² V⁻¹ s⁻¹. The proposed method with general applicability has great potential to be developed as a platform for the growth of high‐quality 2DMCs on the target substrate.

中文翻译：

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表面Marangoni流动诱导靶基板上超薄2D分子晶体的生长

二维分子晶体（2DMC）由于其提高的电荷传输效率和长程分子有序化，正成为有机场效应晶体管（OFET）应用的极佳候选者。但是，当前许多方法都涉及额外的传输过程，这在很大程度上阻碍了在实际应用中大面积制造高质量，完整的2DMC。在此，开发了一种有效的表面Marangoni流致自组装（SMFIS）方法，无需转移过程即可直接在目标基板上制造2DMC。该方法利用溶剂/反溶剂系统将结晶场限制在液/气界面，然后在完全溶剂蒸发的情况下，形成的2DMC降落在目标基板上。通过控制垂直对流和溶剂/反溶剂系统的扩散系数，可以在目标基板上直接生产几层（3-4层）的2DMC。SMFIS方法显示没有基材依赖性和通用兼容性。以双（三乙基甲硅烷基乙炔基）蒽噻吩（Dif-TES-ADT）为例，所得2D Dif-TES-ADT晶体具有有效的电荷传输能力，平均迁移率高达2.15 cm² V ^-1 s ^-1。所提出的具有普遍适用性的方法具有很大的潜力，可以作为在目标基板上生长高质量2DMC的平台。